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1.
Env Sci Adv ; 3(5): 751-762, 2024 May 07.
Article in English | MEDLINE | ID: mdl-38721024

ABSTRACT

Polycyclic aromatic hydrocarbons (PAHs) pose health risks to children, potentially resulting in stunted growth, obesity, and cognitive deficits, but lack of reliable and noninvasive means to measure PAHs results in poor understanding of exposure patterns and sources in this vulnerable population. In this study, 24 children aged ∼7 years (9 boys and 15 girls) from Montevideo, Uruguay wore silicone wristbands for 8 days to monitor the exposure of 27 PAHs. Wristbands were extracted using a modified ethyl acetate tandem solid phase extraction clean up and then analyzed via gas chromatography with tandem mass spectrometry. This analysis has reported LODs for 27 PAHs between 0.05 and 3.91 µg L-1. Eighteen PAHs were detected in >50% of the samples with concentration medians ranging 1.2-16.3 ng g-1 of wristband. Low molecular weight PAHs (2-3 rings) such as naphthalene and its alkyl derivatives were highly correlated (0.7-0.9) in the wristbands, suggesting exposure from related sources. Exposure source exploration focused on secondhand tobacco smoke, potentially through caregivers who reported on smoking habits in an associated survey. A principal components analysis (PCA) was conducted to examine patterns in PAH compounds detected in the wristbands; subsequently, the resulting components were compared according to current smoking among caregivers. The PCA analysis revealed a grouping of participants based on higher exposure of 1-methyl naphthalene, pyrene, fluoranthene, 1-methylphenanthrene, dibenzothiophene and 2-phenyl naphthalene. The derived components did relate with parental smoking, suggesting that some participants experienced exposure to a common source of certain PAHs outside of parental smoking. This is the first study to assess PAH exposure in young children from South America. Using wristbands, our study indicates exposure to multiple, potentially harmful chemicals. Wristbands could provide a comprehensive picture of PAH exposure in children, complementing other non-invasive biomonitoring approaches.

2.
Rapid Commun Mass Spectrom ; 35(8): e9048, 2021 Apr 30.
Article in English | MEDLINE | ID: mdl-33444483

ABSTRACT

RATIONALE: Silicone wristbands have emerged as valuable passive samplers for monitoring of personal exposure to environmental contaminants in the rapidly developing field of exposomics. Once deployed, silicone wristbands collect and hold a wealth of chemical information that can be interrogated using high-resolution mass spectrometry (HRMS) to provide a broad coverage of chemical mixtures. METHODS: Gas chromatography coupled to Orbitrap™ mass spectrometry (GC/Orbitrap™ MS) was used to simultaneously perform suspect screening (using in-house database) and unknown screening (using vendor databases) of extracts from wristbands worn by volunteers. The goal of this study was to optimize a workflow that allows detection of low levels of priority pollutants, with high reliability. In this regard, a data processing workflow for GC/Orbitrap™ MS was developed using a mixture of 123 environmentally relevant standards consisting of pesticides, flame retardants, organophosphate esters, and polycyclic aromatic hydrocarbons as test compounds. RESULTS: The optimized unknown screening workflow using a search index threshold of 750 resulted in positive identification of 70 analytes in validation samples, and a reduction in the number of false positives by over 50%. An average of 26 compounds with high confidence identification, 7 level 1 compounds and 19 level 2 compounds, were observed in worn wristbands. The data were further analyzed via suspect screening and retrospective suspect screening to identify an additional 36 compounds. CONCLUSIONS: This study provides three important findings: (1) a clear evidence of the importance of sample cleanup in addressing complex sample matrices for unknown analysis, (2) a valuable workflow for the identification of unknown contaminants in silicone wristband samplers using electron ionization HRMS data, and (3) a novel application of GC/Orbitrap™ MS for the unknown analysis of organic contaminants that can be used in exposomics studies.


Subject(s)
Environmental Monitoring/instrumentation , Gas Chromatography-Mass Spectrometry/methods , Silicones , Environmental Exposure/analysis , Environmental Monitoring/methods , Environmental Pollutants/analysis , Flame Retardants/analysis , Gas Chromatography-Mass Spectrometry/instrumentation , Humans , Organophosphates/analysis , Pesticides/analysis , Sensitivity and Specificity , Workflow
3.
Sci Total Environ ; 740: 140136, 2020 Oct 20.
Article in English | MEDLINE | ID: mdl-32927574

ABSTRACT

Children are exposed to many potentially toxic compounds in their daily lives and are vulnerable to the harmful effects. To date, very few non-invasive methods are available to quantify children's exposure to environmental chemicals. Due to their ease of implementation, silicone wristbands have emerged as passive samplers to study personal environmental exposures and have the potential to greatly increase our knowledge of chemical exposures in vulnerable population groups. Nevertheless, there is a limited number of studies monitoring children's exposures via silicone wristbands. In this study, we implemented this sampling technique in ongoing research activities in Montevideo, Uruguay which aim to monitor chemical exposures in a cohort of elementary school children. The silicone wristbands were worn by 24 children for 7 days; they were quantitatively analyzed using gas chromatography with tandem mass spectrometry for 45 chemical pollutants, including polychlorinated biphenyls (PCBs), pesticides, polybrominated diphenyl ethers (PBDEs), organophosphorus flame retardants (OPFRs), and novel halogenated flame-retardant chemicals (NHFRs). All classes of chemicals, except NHFRs, were identified in the passive samplers. The average number of analytes detected in each wristband was 13 ±3. OPFRs were consistently the most abundant class of analytes detected. Median concentrations of ΣOPFRs, ΣPBDEs, ΣPCBs, and dichlorodiphenyltrichloroethane (DDT) and its metabolites (dichlorodiphenyldichloroethylene (DDE) and dichlorodiphenyldichloroethane (DDD)) were 1020, 3.00, 0.52 and 3.79 ng/g wristband, respectively. Two major findings result from this research; differences in trends of two OPFRs (TCPP and TDCPP) are observed between studies in Uruguay and the United States, and the detection of DDT, a chemical banned in several countries, suggests that children's exposure profiles in these settings may differ from other parts of the world. This was the first study to examine children's exposome in South America using silicone wristbands and clearly points to a need for further studies.


Subject(s)
Environmental Pollutants , Flame Retardants/analysis , Pesticides , Child , Environmental Monitoring , Halogenated Diphenyl Ethers/analysis , Humans , Organophosphates , Silicones , South America , Uruguay
4.
Environ Int ; 144: 106065, 2020 11.
Article in English | MEDLINE | ID: mdl-32891920

ABSTRACT

Persistent organic pollutants (POPs) accumulate in the food web of the Great Lakes ecosystem, causing concern that these chemicals play a role in the decline of avian species such as colonial-nesting waterbirds. In this study, samples from four life stages of the common tern (Sterna hirundo), a threatened species in New York State, were collected post-mortem in the Buffalo-Niagara region (United States). Brains (n = 26) and livers (n =27) were analyzed for polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), and the insecticide p,p'-dichlorodiphenyltrichloroethane (DDT) and its two metabolites p,p'-dichlorodiphenyldichloroethylene (DDE) and p,p'-dichlorodiphenyldichloroethane (DDD). Detectable concentrations of PCBs and PBDEs were observed in all samples; concentrations of total PCBs ranged from 5.59 to 2,490 ng/g wet weight (ww), total PBDEs ranged from 1.09 to 494 ng/g ww, and DDE metabolites ranged from 0.56 to 637 ng/g ww. Analysis of the primary food source for terns in the Buffalo-Niagara region, emerald shiners (Notropis atherinoides), revealed that all three classes of POPs had similar contaminant profiles in the fish to those in the brains and livers of tern samples. Overall, small chicks contained greater concentrations of pollutants than medium chicks and juveniles, likely from maternal loading to eggs. These results underline the persistence of these legacy contaminants in the Great Lakes, despite their banning, and their biomagnification in threatened species through food web interactions.


Subject(s)
Charadriiformes , Environmental Pollutants , Polychlorinated Biphenyls , Animals , Ecosystem , Environmental Monitoring , Environmental Pollutants/analysis , Halogenated Diphenyl Ethers/analysis , Lakes , New York , Persistent Organic Pollutants , Polychlorinated Biphenyls/analysis
5.
Acta Crystallogr E Crystallogr Commun ; 72(Pt 5): 639-42, 2016 May 01.
Article in English | MEDLINE | ID: mdl-27308008

ABSTRACT

In the title 1:1 co-crystal, C12H10N2·C8H7NO4, the bi-pyridine moiety shows whole-mol-ecule disorder over two sets of sites in a 0.588 (3): 0.412 (3) ratio. In the crystal, the components form hydrogen-bonded sheets linked by N-H⋯O and O-H⋯N inter-actions, which stack along the a axis. A comparison to a related and previously published co-crystal of 5-amino-isophthalic acid and the shorter 4,4'-bipryidine is presented.

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